Atomistic simulation of vibrational strong light-matter interactions*

Here, we introduce how to run classical atomisitic simulation under vibrational strong coupling (VSC), i.e., when a vibrational mode of a large ensemble of realistic molecules is strongly coupled to a cavity mode. This cavity molecular dynamcis (CavMD) scheme not only recover optical spectrum such as the asymmetric Rabi splitting, but also demonstrate many intriguing nonequilibrium dynamics such as vibrational polariton relaxation and polariton-enhanced multiphoton absorption, which can be used to diectly compare with or predict VSC experiments in Fabry-Perot mirocavities.